Dispersionless orbital excitations in (Li,Fe)OHFeSe superconductors

The superconducting critical temperature $T_{\mathrm{c}}$ of intercalated iron-selenide superconductor (Li,Fe)OHFeSe (FeSe11111) can be increased to 42 K from 8 K of bulk FeSe. It shows remarkably similar electronic properties as the high-$T_{\mathrm{c}}$ monolayer FeSe and provides a bulk counterpart to investigate the origin of enhanced superconductivity. Unraveling the nature of collective excitations is crucial for understanding the pairing mechanism in high-$T_{\mathrm{c}}$ iron selenides. Here we use resonant inelastic x-ray scattering (RIXS) to investigate the collective excitations in FeSe11111. Our high-quality data exhibit several Raman-like excitations, which are dispersionless and isotropic in momentum transfer and robust against varying $T_{\mathrm{c}}$. Our RIXS spectra differ much from that of bulk FeSe, but highly resemble that of monolayer FeSe. Using atomic multiplet calculations, we assign the low-energy $\sim 0.3$ and 0.7 eV Raman peaks as local $e_g-e_g$ and $e_g-t_{2g}$ orbital excitations involving spin flips in distorted tetrahedral crystal field. A broad, 2.5 eV high-energy peak is associated with multiplet spin interactions. Our results highlight the importance of both orbital and spin degrees of freedom in the pairing of high-$T_{\mathrm{c}}$ iron selenides.